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Over the last few decades, nonlinear optics has become significantly more nonlinear, traversing nearly a billionfold improvement in energy efficiency, with ultrafast nonlinear nanophotonics in particular emerging as a frontier for combining both spatial and temporal engineering. At present, cutting-edge experiments in nonlinear nanophotonics place us just above themesoscopicregime, where a few hundred photons suffice to trigger highly nonlinear dynamics. In contrast to classical or deep-quantum optics, the mesoscale is characterized by dynamical interactions between mean-field, Gaussian, and non-Gaussian quantum features, all within a close hierarchy of scales. When combined with the inherent multimode complexity of optical fields, such hybrid quantum-classical dynamics present theoretical, experimental, and engineering challenges to the contemporary framework of quantum optics. In this review, we highlight the unique physics that emerges in multimode nonlinear optics at the mesoscale and outline key principles for exploiting both classical and quantum features to engineer novel functionalities. We briefly survey the experimental landscape and draw attention to outstanding technical challenges in materials, dispersion engineering, and device design for accessing mesoscopic operation. Finally, we speculate on how these capabilities might usher in some new paradigms in quantum photonics, from quantum-augmented information processing to nonclassical-light-driven dynamics and phenomena to all-optical non-Gaussian measurement and sensing. The physics unlocked at the mesoscale present significant challenges and opportunities in theory and experiment alike, and this review is intended to serve as a guide to navigating this new frontier in ultrafast quantum nonlinear optics.

Photonic integrated circuits with second-order (χ⁽²⁾) nonlinearities are rapidly scaling to remarkably low powers. At this time, state-of-the-art devices achieve saturated nonlinear interactions with thousands of photons when driven by continuous-wave lasers, and further reductions in these energy requirements enabled by the use of ultrafast pulses may soon push nonlinear optics into the realm of single-photon nonlinearities. This tutorial reviews these recent developments in ultrafast nonlinear photonics, discusses design strategies for realizing few-photon nonlinear interactions, and presents a unified treatment of ultrafast quantum nonlinear optics using a framework that smoothly interpolates from classical behaviors to the few-photon scale. These emerging platforms for quantum optics fundamentally differ from typical realizations in cavity quantum electrodynamics due to the large number of coupled optical modes. Classically, multimode behaviors have been well studied in nonlinear optics, with famous examples including soliton formation and supercontinuum generation. In contrast, multimode quantum systems exhibit a far greater variety of behaviors, and yet closed-form solutions are even sparser than their classical counterparts. In developing a framework for ultrafast quantum optics, we identify what behaviors carry over from classical to quantum devices, what intuition must be abandoned, and what new opportunities exist at the intersection of ultrafast and quantum nonlinear optics. Although this article focuses on establishing connections between the classical and quantum behaviors of devices withχ⁽²⁾nonlinearities, the frameworks developed here are general and are readily extended to the description of dynamical processes based on third-orderχ⁽³⁾nonlinearities.

Silicon is a common material for photonics due to its favorable optical properties in the telecom and mid-wave IR bands, as well as compatibility with a wide range of complementary metal–oxide semiconductor (CMOS) foundry processes. Crystalline inversion symmetry precludes silicon from natively exhibiting second-order nonlinear optical processes. In this work, we build on recent works in silicon photonics that break this material symmetry using large bias fields, thereby enablingχ⁽²⁾interactions. Using this approach, we demonstrate both second-harmonic generation (with a normalized efficiency of 0.20%W⁻¹cm⁻²) and, to our knowledge, the first degenerateχ⁽²⁾optical parametric amplifier (with an estimated normalized gain of 0.6dBW^−1/2cm⁻¹) using silicon-on-insulator waveguides fabricated in a CMOS-compatible commercial foundry. We expect this technology to enable the integration of novel nonlinear optical devices such as optical parametric amplifiers, oscillators, and frequency converters into large-scale, hybrid photonic–electronic systems by leveraging the extensive ecosystem of CMOS fabrication.

The realization of deterministic photon–photon gates is a central goal in optical quantum computation and engineering. A longstanding challenge is that optical nonlinearities in scalable, room-temperature material platforms are too weak to achieve the required strong coupling, due to the critical loss-confinement trade-off in existing photonic structures. In this work, we introduce a spatio-temporal confinement method, dispersion-engineered temporal trapping, to circumvent the trade-off, enabling a route to all-optical strong coupling. Temporal confinement is imposed by an auxiliary trap pulse via cross-phase modulation, which, combined with the spatial confinement of a waveguide, creates a “flying cavity” that enhances the nonlinear interaction strength by at least an order of magnitude. Numerical simulations confirm that temporal trapping confines the multimode nonlinear dynamics to a single-mode subspace, enabling high-fidelity deterministic quantum gate operations. With realistic dispersion engineering and loss figures, we show that temporally trapped ultrashort pulses could achieve strong coupling on near-term nonlinear nanophotonic platforms. Our results highlight the potential of ultrafast nonlinear optics to become the first scalable, high-bandwidth, and room-temperature platform that achieves strong coupling, opening a path to quantum computing, simulation, and light sources.

Thin-film lithium niobate (TFLN) is an emerging platform for compact, low-power nonlinear-optical devices, and has been used extensively for near-infrared frequency conversion. Recent work has extended these devices to mid-infrared wavelengths, where broadly tunable sources may be used for chemical sensing. To this end, we demonstrate efficient and broadband difference frequency generation between a fixed 1-µm pump and a tunable telecom source in uniformly-poled TFLN-on-sapphire by harnessing the dispersion-engineering available in tightly-confining waveguides. We show a simultaneous 1–2 order-of-magnitude improvement in conversion efficiency and ∼5-fold enhancement of operating bandwidth for mid-infrared generation when compared to equal-length conventional lithium niobate waveguides. We also examine the effects of mid-infrared loss from surface-adsorbed water on the performance of these devices.

We study the emergence of non-Gaussian quantum features in pulsed squeezed light generation with a mesoscopic number (i.e., dozens to hundreds) of pump photons. Due to the strong optical nonlinearities necessarily involved in this regime, squeezing occurs alongside significant pump depletion, compromising the predictions made by conventional semiclassical models for squeezing. Furthermore, nonlinear interactions among multiple frequency modes render the system dynamics exponentially intractable in naïve quantum models, requiring a more sophisticated modeling framework. To this end, we construct a nonlinear Gaussian approximation to the squeezing dynamics, defining a “Gaussian interaction frame” in which non-Gaussian quantum dynamics can be isolated and concisely described using a few dominant (i.e., principal) supermodes. Numerical simulations of our model reveal non-Gaussian distortions of squeezing in the mesoscopic regime, largely associated with signal-pump entanglement. We argue that state of the art in nonlinear nanophotonics is quickly approaching this regime, providing an all-optical platform for experimental studies of the semiclassical-to-quantum transition in a rich paradigm of coherent, multimode nonlinear dynamics. Mesoscopic pulsed squeezing, thus, provides an intriguing case study of the rapid rise in dynamic complexity associated with semiclassical-to-quantum crossover, which we view as a correlate of the emergence of new information processing capacities in the quantum regime.

Ultrashort pulses propagating in nonlinear nanophotonic waveguides can simultaneously leverage both temporal and spatial field confinement, promising a route towards single-photon nonlinearities in an all-photonic platform. In this multimode quantum regime, however, faithful numerical simulations of pulse dynamics naïvely require a representation of the state in an exponentially large Hilbert space. Here, we employ a time-domain, matrix product state (MPS) representation to enable efficient simulations by exploiting the entanglement structure of the system. To extract physical insight from these simulations, we develop an algorithm to unravel the MPS quantum state into constituent temporal supermodes, enabling, e.g., access to the phase-space portraits of arbitrary pulse waveforms. As a demonstration, we perform exact numerical simulations of a Kerr soliton in the quantum regime. We observe the development of non-classical Wigner-function negativity in the solitonic mode as well as quantum corrections to the semiclassical dynamics of the pulse. A similar analysis of${\mathrm{\chi <\#comment/>}}^{(2)}$simultons reveals a unique entanglement structure between the fundamental and second harmonics. Our approach is also readily compatible with quantum trajectory theory, allowing full quantum treatment of propagation loss and decoherence. We expect this work to establish the MPS technique as part of a unified engineering framework for the emerging field of broadband quantum photonics.

Periodically poled thin-film lithium niobate (TFLN) waveguides have emerged as a leading platform for highly efficient frequency conversion in the near-infrared. However, the commonly used silica bottom-cladding results in high absorption loss at wavelengths beyond 2.5 µm. In this work, we demonstrate efficient frequency conversion in a TFLN-on-sapphire platform, which features high transparency up to 4.5 µm. In particular, we report generating mid-infrared light up to 3.66 µm via difference-frequency generation of a fixed 1 µm source and a tunable telecom source, with normalized efficiencies up to$200\mathrm{\%<\#comment/>}/\mathrm{W}{\mathrm{c}\mathrm{m}}^2$. These results show TFLN-on-sapphire to be a promising platform for integrated nonlinear nanophotonics in the mid-infrared.